EP3727653A1 - Filtre à particules à activité catalytique - Google Patents

Filtre à particules à activité catalytique

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Publication number
EP3727653A1
EP3727653A1 EP18816073.3A EP18816073A EP3727653A1 EP 3727653 A1 EP3727653 A1 EP 3727653A1 EP 18816073 A EP18816073 A EP 18816073A EP 3727653 A1 EP3727653 A1 EP 3727653A1
Authority
EP
European Patent Office
Prior art keywords
zirconium
rare earth
cerium
oxide
particulate filter
Prior art date
Legal status (The legal status is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the status listed.)
Granted
Application number
EP18816073.3A
Other languages
German (de)
English (en)
Other versions
EP3727653B1 (fr
Inventor
Jan Schoenhaber
Naina DEIBEL
Martin Roesch
Stephanie SPIESS
Meike GOTTHARDT
Nicole SCHICHTEL
Current Assignee (The listed assignees may be inaccurate. Google has not performed a legal analysis and makes no representation or warranty as to the accuracy of the list.)
Umicore AG and Co KG
Original Assignee
Umicore AG and Co KG
Priority date (The priority date is an assumption and is not a legal conclusion. Google has not performed a legal analysis and makes no representation as to the accuracy of the date listed.)
Filing date
Publication date
Application filed by Umicore AG and Co KG filed Critical Umicore AG and Co KG
Priority to EP23212574.0A priority Critical patent/EP4365421A3/fr
Publication of EP3727653A1 publication Critical patent/EP3727653A1/fr
Application granted granted Critical
Publication of EP3727653B1 publication Critical patent/EP3727653B1/fr
Active legal-status Critical Current
Anticipated expiration legal-status Critical

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Classifications

    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
    • B01D53/34—Chemical or biological purification of waste gases
    • B01D53/92—Chemical or biological purification of waste gases of engine exhaust gases
    • B01D53/94—Chemical or biological purification of waste gases of engine exhaust gases by catalytic processes
    • B01D53/9445—Simultaneously removing carbon monoxide, hydrocarbons or nitrogen oxides making use of three-way catalysts [TWC] or four-way-catalysts [FWC]
    • B01D53/945—Simultaneously removing carbon monoxide, hydrocarbons or nitrogen oxides making use of three-way catalysts [TWC] or four-way-catalysts [FWC] characterised by a specific catalyst
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D53/00—Separation of gases or vapours; Recovering vapours of volatile solvents from gases; Chemical or biological purification of waste gases, e.g. engine exhaust gases, smoke, fumes, flue gases, aerosols
    • B01D53/34—Chemical or biological purification of waste gases
    • B01D53/92—Chemical or biological purification of waste gases of engine exhaust gases
    • B01D53/94—Chemical or biological purification of waste gases of engine exhaust gases by catalytic processes
    • B01D53/9459—Removing one or more of nitrogen oxides, carbon monoxide, or hydrocarbons by multiple successive catalytic functions; systems with more than one different function, e.g. zone coated catalysts
    • B01D53/9463—Removing one or more of nitrogen oxides, carbon monoxide, or hydrocarbons by multiple successive catalytic functions; systems with more than one different function, e.g. zone coated catalysts with catalysts positioned on one brick
    • B01D53/9468—Removing one or more of nitrogen oxides, carbon monoxide, or hydrocarbons by multiple successive catalytic functions; systems with more than one different function, e.g. zone coated catalysts with catalysts positioned on one brick in different layers
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J21/00—Catalysts comprising the elements, oxides, or hydroxides of magnesium, boron, aluminium, carbon, silicon, titanium, zirconium, or hafnium
    • B01J21/06—Silicon, titanium, zirconium or hafnium; Oxides or hydroxides thereof
    • B01J21/066—Zirconium or hafnium; Oxides or hydroxides thereof
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J23/00—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00
    • B01J23/10—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of rare earths
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J23/00—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00
    • B01J23/38—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of noble metals
    • B01J23/40—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of noble metals of the platinum group metals
    • B01J23/46—Ruthenium, rhodium, osmium or iridium
    • B01J23/464—Rhodium
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J23/00—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00
    • B01J23/38—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of noble metals
    • B01J23/54—Catalysts comprising metals or metal oxides or hydroxides, not provided for in group B01J21/00 of noble metals combined with metals, oxides or hydroxides provided for in groups B01J23/02 - B01J23/36
    • B01J23/56—Platinum group metals
    • B01J23/63—Platinum group metals with rare earths or actinides
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J35/00—Catalysts, in general, characterised by their form or physical properties
    • B01J35/19—Catalysts containing parts with different compositions
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01J—CHEMICAL OR PHYSICAL PROCESSES, e.g. CATALYSIS OR COLLOID CHEMISTRY; THEIR RELEVANT APPARATUS
    • B01J35/00—Catalysts, in general, characterised by their form or physical properties
    • B01J35/50—Catalysts, in general, characterised by their form or physical properties characterised by their shape or configuration
    • B01J35/56—Foraminous structures having flow-through passages or channels, e.g. grids or three-dimensional monoliths
    • F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F01—MACHINES OR ENGINES IN GENERAL; ENGINE PLANTS IN GENERAL; STEAM ENGINES
    • F01N—GAS-FLOW SILENCERS OR EXHAUST APPARATUS FOR MACHINES OR ENGINES IN GENERAL; GAS-FLOW SILENCERS OR EXHAUST APPARATUS FOR INTERNAL COMBUSTION ENGINES
    • F01N3/00—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust
    • F01N3/02—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust for cooling, or for removing solid constituents of, exhaust
    • F01N3/021—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust for cooling, or for removing solid constituents of, exhaust by means of filters
    • F01N3/033—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust for cooling, or for removing solid constituents of, exhaust by means of filters in combination with other devices
    • F01N3/035—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust for cooling, or for removing solid constituents of, exhaust by means of filters in combination with other devices with catalytic reactors, e.g. catalysed diesel particulate filters
    • F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F01—MACHINES OR ENGINES IN GENERAL; ENGINE PLANTS IN GENERAL; STEAM ENGINES
    • F01N—GAS-FLOW SILENCERS OR EXHAUST APPARATUS FOR MACHINES OR ENGINES IN GENERAL; GAS-FLOW SILENCERS OR EXHAUST APPARATUS FOR INTERNAL COMBUSTION ENGINES
    • F01N3/00—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust
    • F01N3/08—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust for rendering innocuous
    • F01N3/10—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust for rendering innocuous by thermal or catalytic conversion of noxious components of exhaust
    • F01N3/101—Three-way catalysts
    • F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F01—MACHINES OR ENGINES IN GENERAL; ENGINE PLANTS IN GENERAL; STEAM ENGINES
    • F01N—GAS-FLOW SILENCERS OR EXHAUST APPARATUS FOR MACHINES OR ENGINES IN GENERAL; GAS-FLOW SILENCERS OR EXHAUST APPARATUS FOR INTERNAL COMBUSTION ENGINES
    • F01N3/00—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust
    • F01N3/08—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust for rendering innocuous
    • F01N3/10—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust for rendering innocuous by thermal or catalytic conversion of noxious components of exhaust
    • F01N3/24—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust for rendering innocuous by thermal or catalytic conversion of noxious components of exhaust characterised by constructional aspects of converting apparatus
    • F01N3/28—Construction of catalytic reactors
    • F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F01—MACHINES OR ENGINES IN GENERAL; ENGINE PLANTS IN GENERAL; STEAM ENGINES
    • F01N—GAS-FLOW SILENCERS OR EXHAUST APPARATUS FOR MACHINES OR ENGINES IN GENERAL; GAS-FLOW SILENCERS OR EXHAUST APPARATUS FOR INTERNAL COMBUSTION ENGINES
    • F01N3/00—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust
    • F01N3/08—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust for rendering innocuous
    • F01N3/10—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust for rendering innocuous by thermal or catalytic conversion of noxious components of exhaust
    • F01N3/24—Exhaust or silencing apparatus having means for purifying, rendering innocuous, or otherwise treating exhaust for rendering innocuous by thermal or catalytic conversion of noxious components of exhaust characterised by constructional aspects of converting apparatus
    • F01N3/28—Construction of catalytic reactors
    • F01N3/2803—Construction of catalytic reactors characterised by structure, by material or by manufacturing of catalyst support
    • F01N3/2825—Ceramics
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D2255/00—Catalysts
    • B01D2255/10—Noble metals or compounds thereof
    • B01D2255/102—Platinum group metals
    • B01D2255/1021—Platinum
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D2255/00—Catalysts
    • B01D2255/10—Noble metals or compounds thereof
    • B01D2255/102—Platinum group metals
    • B01D2255/1023—Palladium
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D2255/00—Catalysts
    • B01D2255/10—Noble metals or compounds thereof
    • B01D2255/102—Platinum group metals
    • B01D2255/1025—Rhodium
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D2255/00—Catalysts
    • B01D2255/20—Metals or compounds thereof
    • B01D2255/206—Rare earth metals
    • B01D2255/2061—Yttrium
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D2255/00—Catalysts
    • B01D2255/20—Metals or compounds thereof
    • B01D2255/206—Rare earth metals
    • B01D2255/2063—Lanthanum
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D2255/00—Catalysts
    • B01D2255/20—Metals or compounds thereof
    • B01D2255/206—Rare earth metals
    • B01D2255/2065—Cerium
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D2255/00—Catalysts
    • B01D2255/20—Metals or compounds thereof
    • B01D2255/206—Rare earth metals
    • B01D2255/2066—Praseodymium
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D2255/00—Catalysts
    • B01D2255/20—Metals or compounds thereof
    • B01D2255/207—Transition metals
    • B01D2255/20715—Zirconium
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
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    • B01D2255/00—Catalysts
    • B01D2255/20—Metals or compounds thereof
    • B01D2255/209—Other metals
    • B01D2255/2092—Aluminium
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D2255/00—Catalysts
    • B01D2255/40—Mixed oxides
    • B01D2255/407—Zr-Ce mixed oxides
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D2255/00—Catalysts
    • B01D2255/90—Physical characteristics of catalysts
    • B01D2255/902—Multilayered catalyst
    • B01D2255/9022—Two layers
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D2255/00—Catalysts
    • B01D2255/90—Physical characteristics of catalysts
    • B01D2255/908—O2-storage component incorporated in the catalyst
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D2255/00—Catalysts
    • B01D2255/90—Physical characteristics of catalysts
    • B01D2255/915—Catalyst supported on particulate filters
    • B01D2255/9155—Wall flow filters
    • B—PERFORMING OPERATIONS; TRANSPORTING
    • B01—PHYSICAL OR CHEMICAL PROCESSES OR APPARATUS IN GENERAL
    • B01D—SEPARATION
    • B01D2258/00—Sources of waste gases
    • B01D2258/01—Engine exhaust gases
    • B01D2258/014—Stoichiometric gasoline engines
    • F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F01—MACHINES OR ENGINES IN GENERAL; ENGINE PLANTS IN GENERAL; STEAM ENGINES
    • F01N—GAS-FLOW SILENCERS OR EXHAUST APPARATUS FOR MACHINES OR ENGINES IN GENERAL; GAS-FLOW SILENCERS OR EXHAUST APPARATUS FOR INTERNAL COMBUSTION ENGINES
    • F01N2330/00—Structure of catalyst support or particle filter
    • F01N2330/06—Ceramic, e.g. monoliths
    • F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F01—MACHINES OR ENGINES IN GENERAL; ENGINE PLANTS IN GENERAL; STEAM ENGINES
    • F01N—GAS-FLOW SILENCERS OR EXHAUST APPARATUS FOR MACHINES OR ENGINES IN GENERAL; GAS-FLOW SILENCERS OR EXHAUST APPARATUS FOR INTERNAL COMBUSTION ENGINES
    • F01N2330/00—Structure of catalyst support or particle filter
    • F01N2330/30—Honeycomb supports characterised by their structural details
    • F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F01—MACHINES OR ENGINES IN GENERAL; ENGINE PLANTS IN GENERAL; STEAM ENGINES
    • F01N—GAS-FLOW SILENCERS OR EXHAUST APPARATUS FOR MACHINES OR ENGINES IN GENERAL; GAS-FLOW SILENCERS OR EXHAUST APPARATUS FOR INTERNAL COMBUSTION ENGINES
    • F01N2370/00—Selection of materials for exhaust purification
    • F01N2370/02—Selection of materials for exhaust purification used in catalytic reactors
    • F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F01—MACHINES OR ENGINES IN GENERAL; ENGINE PLANTS IN GENERAL; STEAM ENGINES
    • F01N—GAS-FLOW SILENCERS OR EXHAUST APPARATUS FOR MACHINES OR ENGINES IN GENERAL; GAS-FLOW SILENCERS OR EXHAUST APPARATUS FOR INTERNAL COMBUSTION ENGINES
    • F01N2510/00—Surface coverings
    • F01N2510/06—Surface coverings for exhaust purification, e.g. catalytic reaction
    • F—MECHANICAL ENGINEERING; LIGHTING; HEATING; WEAPONS; BLASTING
    • F01—MACHINES OR ENGINES IN GENERAL; ENGINE PLANTS IN GENERAL; STEAM ENGINES
    • F01N—GAS-FLOW SILENCERS OR EXHAUST APPARATUS FOR MACHINES OR ENGINES IN GENERAL; GAS-FLOW SILENCERS OR EXHAUST APPARATUS FOR INTERNAL COMBUSTION ENGINES
    • F01N2510/00—Surface coverings
    • F01N2510/06—Surface coverings for exhaust purification, e.g. catalytic reaction
    • F01N2510/068—Surface coverings for exhaust purification, e.g. catalytic reaction characterised by the distribution of the catalytic coatings
    • F01N2510/0684—Surface coverings for exhaust purification, e.g. catalytic reaction characterised by the distribution of the catalytic coatings having more than one coating layer, e.g. multi-layered coatings
    • Y—GENERAL TAGGING OF NEW TECHNOLOGICAL DEVELOPMENTS; GENERAL TAGGING OF CROSS-SECTIONAL TECHNOLOGIES SPANNING OVER SEVERAL SECTIONS OF THE IPC; TECHNICAL SUBJECTS COVERED BY FORMER USPC CROSS-REFERENCE ART COLLECTIONS [XRACs] AND DIGESTS
    • Y02—TECHNOLOGIES OR APPLICATIONS FOR MITIGATION OR ADAPTATION AGAINST CLIMATE CHANGE
    • Y02T—CLIMATE CHANGE MITIGATION TECHNOLOGIES RELATED TO TRANSPORTATION
    • Y02T10/00—Road transport of goods or passengers
    • Y02T10/10—Internal combustion engine [ICE] based vehicles
    • Y02T10/12—Improving ICE efficiencies

Definitions

  • the present invention relates to a catalytically active particulate filter which is particularly suitable for the removal of particles, carbon monoxide, hydrocarbons and nitrogen oxides from the exhaust gas of stoichiometric air / fuel mixture operated internal combustion engines.
  • Gasoline engines are cleaned in conventional processes using three-way catalysts. These are able to absorb the three main gaseous pollutants of the engine, namely hydrocarbons,
  • Combustion air ratio l (A / F ratio, air / fuel ratio) sets the actual air mass m L, tats available for combustion in relation to the stoichiometric air mass m i_, st:
  • the particles in the exhaust gas of stoichiometrically operated internal combustion engines are very small and have one average particle size less than 1 pm. Typical particle sizes range from 10 nm to 200 nm. Furthermore, the amount of particles emitted is very small and ranges from 2 mg / km to 4 mg / km.
  • WLTP harmonized light vehicle test cycle
  • wall flow filters In the field of purification of exhaust gas from lean-burn engines, ie in particular diesel engines, wall flow filters have
  • ceramic materials e.g. Silicon carbide, aluminum titanate and cordierite proven. These are composed of a plurality of parallel channels formed by porous walls.
  • the channels are mutually closed at one of the two ends of the filter to form channels A which are open on the first side of the filter and closed on the second side of the filter, and channels B which are closed on the first side of the filter and are open on the second side of the filter.
  • the exhaust gas flowing, for example, into the channels A can leave the filter only via the channels B, and must flow through the porous walls between the channels A and B for this purpose. As the exhaust gas passes through the wall, the particles are retained and the exhaust gas purified.
  • the wall-flow filter is provided with catalytically active coatings which reduce the ignition temperature of soot. It is already known to apply such coatings to the porous walls between the channels (so-called on-wall coating) or to introduce them into the porous walls (so-called in-wall coating).
  • EP 1657410 A2 also already describes a
  • one part of the catalytically active material is present in the porous walls and another part on the porous walls.
  • a wall flow filter carries two superposed layers, one in the porous wall and the other on the porous wall.
  • porous filter walls contain a catalyst material of a three-way catalyst, while in addition a catalyst material of a three-way catalyst is applied to portions of the filter walls.
  • FR 3020091 A1 discloses a particulate filter which carries a coating in the porous walls as well as coatings on the surfaces of the input and output channels. The latter extend over a portion of the filter length, both to the input and to the filter
  • the filter should have the lowest possible back pressure, so that the engine power is maintained and the lowest possible fuel consumption can be realized.
  • the present invention relates to a particulate filter for removing particulates, carbon monoxide, hydrocarbons and nitrogen oxides from the exhaust gas of stoichiometric air / fuel mixture operated internal combustion engines, the wall flow filter of length L and a
  • the wall flow filter comprises channels E and A extending in parallel between a first and a second end of the
  • Wall flow filters and which are separated by porous walls forming surfaces OE and OA and wherein the channels E at the second end and the channels A are closed at the first end, characterized in that coating Z is in the porous walls and starting extending from the first end of the wall flow filter over the length L and active alumina, at least, preferably two different cerium / zirconium / rare earth metal mixed oxides and at least one platinum group metal.
  • the coating Z is catalytically active, especially at
  • Oxygen storage components differ with respect to at least one of the contained Components. Like constituents of the oxygen storage materials may be contained in equal or different amounts.
  • oxygen storage components are cerium / zirconium / rare earth metal mixed oxides.
  • cerium / zirconium / rare earth metal mixed oxides are particularly suitable oxygen storage components.
  • cerium / zirconium / rare earth mixed oxides are characterized by a substantially homogeneous, three-dimensional crystal structure which is ideally free of phases of pure ceria, zirconia or rare earth oxide.
  • products which are not completely homogeneous to form which as a rule can be used without disadvantage.
  • rare earth metal or rare earth metal oxide does not include cerium or cerium oxide.
  • rare earth metal oxides in the cerium / zirconium / rare earth metal mixed oxides are lanthanum oxide, yttrium oxide, praseodymium oxide,
  • Neodymium oxide and / or samarium oxide into consideration.
  • Lanthanum oxide, yttrium oxide and / or praseodymium oxide are preferred.
  • Lanthanum oxide and / or yttrium oxide are particularly preferred in this context as rare earth metals, and very particular preference is given to lanthanum oxide and yttrium oxide, yttrium oxide and
  • Praseodymium oxide as well as lanthanum oxide and praseodymium oxide.
  • the oxygen storage components are free of neodymium oxide.
  • the weight ratio of alumina is the sum of the two
  • Cerium / zirconium / rare earth mixed oxides ranges from 10:90 to 60:40, preferably in the range of from 20:80 to 50:50, and more preferably in the range of from 25:75 to 35:65.
  • the coating Z comprises in preferred embodiments in each case lanthanum-stabilized
  • Alumina in amounts of 10 to 60 wt .-%, preferably 20 to 50, particularly preferably 25 to 35 wt .-%, and
  • Oxygen storage components in amounts of 40 to 90 wt .-%, preferably 50 to 80 wt .-%, particularly preferably 65 to 75 wt .-%, each based on the sum of the weights of alumina and oxygen storage components in the coating Z.
  • the coating Z in embodiments preferably comprises two different oxygen storage components, wherein the weight ratio of the first cerium / zirconium / rare earth mixed oxide to the second cerium / zirconium / rare earth mixed oxide is in the range of 4: 1 to 1: 4, preferably in the range of 3: 1 to 1: 3 and more preferably in the range of 2: 1 to 1: 2.
  • coating Z comprises first and second oxygen storage components, wherein the first oxygen storage component has a higher zirconium oxide content than the second oxygen storage component.
  • the mass ratio of ceria to zirconia in the cerium / zirconium / rare earth mixed oxides can vary widely. It is for example 0.1 to 1.5, preferably 0.2 to 1.25 or 0.3 to 1. It is further preferred if the first
  • Oxygen storage component has a weight ratio of ceria to zirconia of 0.7 to 0.1, which is smaller than in the second cerium / zirconium / rare earth mixed oxide having a weight ratio of ceria to zirconia of 0.5 to 1.5. More more preferred embodiments include a first
  • Oxygen storage component having a weight ratio of ceria to zirconia of 0.6 to 0.2 and a second
  • Oxygen storage component having a weight ratio of ceria to zirconia of from 0.6 to 1.2. Still others very much preferred
  • Embodiments include a first oxygen storage component having a weight ratio of ceria to zirconia of from 0.5 to 0.3, and the second oxygen storage component has a weight ratio of ceria to zirconia of from 0.7 to 1.0.
  • Particulate filter designed so that the first cerium / zirconium / rare earth mixed oxide a cerium oxide content of 10% to 40% based on the
  • the zirconium oxide content is in the first
  • Cerium / zirconium / rare earth mixed oxide at 40% to 90% by weight of the first cerium / zirconium / rare earth mixed oxide.
  • Cerium / zirconium / rare earth mixed oxide between 50% to 75%, from 55% to 65% by weight of the first
  • Cerium / zirconium / rare earth mixed oxide lies.
  • a cerium oxide content of 25% to 60% based on the weight of the second cerium-zirconium-rare earth mixed oxide should prevail. It is more advantageous if a cerium oxide content of 30% to 55%, more preferably 35% to 50%, based on the weight of the second cerium / zirconium / rare earth metal mixed oxide, is present in the second cerium / zirconium / rare earth metal oxide.
  • the second cerium oxide content of 30% to 55%, more preferably 35% to 50% is present in the second cerium / zirconium / rare earth metal oxide.
  • Cerium / zirconium / rare earth mixed oxide has a zirconia content of 20% to 70% by weight of the second
  • Cerium / zirconium / rare earth mixed oxide is preferable when the second cerium / zirconium / rare earth mixed oxide has a
  • Zirconium oxide content of 30% to 60%, and most preferably from 40% to 55% by weight of the second
  • Cerium / zirconium / rare earth mixed oxide Cerium / zirconium / rare earth mixed oxide.
  • cerium / zirconium / rare earth metal mixed oxides when both cerium / zirconium / rare earth metal mixed oxides are doped with lanthanum, so that preferably the content of lanthanum oxide> 0% to 10% based on the weight of
  • Cerium / zirconium / rare earth mixed oxide These lanthanum oxide-containing oxygen storage components particularly advantageously have a mass ratio of lanthanum oxide to cerium oxide of 0.05 to 0.5.
  • coating Z comprises lanthanum stabilized alumina, as well as rhodium, palladium or palladium and rhodium, and two different, zirconia, ceria, lanthana, and yttria or praseodymium oxide
  • the first cerium / zirconium / rare earth mixed oxide is doped with yttria in addition to lanthana.
  • a preferred particulate filter has an yttria content in the first cerium / zirconium / rare earth mixed oxide of 2% to 25% by weight of the first
  • Cerium / zirconium / rare earth oxide More preferably, the yttria content of the first cerium / zirconium / rare earth composite oxide is from 4% to 20%, more preferably from 10% to 15% by weight of the first cerium / zirconium / rare earth composite oxide. Also advantageous is an embodiment in which the second
  • Cerium / zirconium / rare earth metal mixed oxide in addition to lanthanum oxide is doped with a further metal oxide from the group of rare earth metal oxides, preferably with praseodymium.
  • the zirconia content of the yttria-containing oxygen storage component is greater than the zirconia content of the zirconia
  • Cerium / zirconium / rare earth mixed oxide may range between 2% to 15% by weight of the second cerium / zirconium / rare earth mixed oxide. It is more advantageous if the content of the second cerium / zirconium / rare earth mixed oxide.
  • Rare earth metal of the second cerium / zirconium / rare earth metal composite oxide is 3% to 10%, more preferably 4% to 8%, based on the weight of the second cerium / zirconium / rare earth metal composite oxide.
  • coating Z is the yttria content of the first
  • Oxygen storage component in particular 5 to 15 wt .-%, based on the weight of the oxygen storage component.
  • the weight ratio of lanthanum oxide to yttrium oxide is in particular 0.1 to 1,
  • the praseodymium content is the second
  • Oxygen storage component in particular 2 to 10 wt .-%, based on the weight of the oxygen storage component.
  • the weight ratio of lanthanum oxide to praseodymium oxide is in particular from 0.1 to 2.0, preferably from 0.2 to 1.8 and very preferably from 0.5 to 1.5.
  • the coating contains Z as catalytically active
  • Rhodium, platinum and rhodium or platinum, palladium and rhodium may be activated.
  • the catalytically active coating is located in the pores of the porous wall of a wall-flow filter. Only small parts can be present on the wall due to the coating process.
  • the coating Z is present to> 95% in the pores of the wall.
  • the noble metals are usually used in amounts of 0.15 g / l to 5 g / l, based on the volume of the wall-flow filter. In a preferred embodiment, the precious metals are both on the
  • Suitable carrier materials for the noble metals are all those skilled in the art for this purpose materials. Such materials are in particular metal oxides having a BET surface area of from 30 to 250 m 2 / g, preferably from 100 to 200 m 2 / g (determined in accordance with DIN 66132 - latest version on the filing date).
  • Particularly suitable support materials for the noble metals are selected from the series consisting of alumina, doped alumina, silica, titania and mixed oxides of one or more thereof.
  • Doped aluminum oxides are, for example, with lanthanum oxide, barium oxide, zirconium oxide and / or titanium oxide-doped aluminum oxides.
  • lanthanum-stabilized alumina is used, wherein lanthanum in amounts of 1 to 10 wt .-%, preferably 3 to 6 wt .-%, each calculated as La2Ü 3 and based on the weight of the stabilized aluminum oxide is used.
  • the coating Z contains oxygen storage components in amounts of 15 to 120 g / l, based on the volume of the wall-flow filter.
  • the mass ratio of carrier materials and oxygen storage components in coating Z is usually 0.2 to 1.5, for example 0.3 to 0.8.
  • coating Z contains one or more alkaline earth compounds, such as e.g. Strontium oxide,
  • Barium oxide or barium sulfate is in particular 2 to 20 g / l volume of the wall-flow filter.
  • coating Z contains strontium oxide or barium oxide.
  • Coating Z additives such as rare earth compounds such. B. lanthanum oxide and / or binders, such as. B. aluminum compounds. These additives are used in amounts which can vary within wide limits and which the skilled person can determine in a concrete case by simple means.
  • the coating Z extends from the first end of the wall-flow filter over the entire length L of the wall-flow filter.
  • the loading of the wall-flow filter with coating Z is preferably 20 to 125 g / l, based on the volume of the
  • coating Z contains no zeolite or molecular sieve.
  • Wall-flow filters which can be used in accordance with the present invention are known and available on the market. They exist, for example silicon carbide, aluminum titanate or cordierite, for example, have a cell density of 200 to 400 cells per square inch (cpsi), ie about 30 to 60 cells per cm 2 , and usually a wall thickness between 6 and 12 mils, and 0.1524 and 0.305, respectively mm.
  • cpsi cells per square inch
  • a wall thickness between 6 and 12 mils, and 0.1524 and 0.305, respectively mm.
  • uncoated state for example, they have porosities of 50 to 80%, in particular 55 to 75%. Their average pore size when uncoated, for example, 10 to 25 microns.
  • the pores of the wall-flow filter are so-called open pores, that is to say they have a connection to the channels. Furthermore, the pores are usually interconnected. This allows, on the one hand, the slight coating of the inner pore surfaces and, on the other hand, an easy passage of the exhaust gas through the porous walls of the wall-flow filter.
  • the production of the particulate filter according to the invention can be carried out by methods familiar to the person skilled in the art, for example by applying a coating suspension, which is usually called washcoat, to the wall-flow filter by means of one of the customary dip-coating methods or pump and suction coating methods.
  • a coating suspension which is usually called washcoat
  • the average pore size of the wallflow filter and the average particle size of the catalytically active materials must be matched to achieve an on-wall or in-wall coating.
  • the average particle size of the catalytically active materials must be small enough to penetrate the pores of the wall-flow filter
  • the average particle size of the catalytically active materials must be large enough not to penetrate into the pores of the wall-flow filter.
  • the particle filter according to the invention is ideal for
  • Nitrogen oxides from the exhaust of operated with stoichiometric air / fuel mixture internal combustion engines are included.
  • the present invention thus also relates to a process for the removal of particles, carbon monoxide, hydrocarbons and nitrogen oxides from the exhaust gas of stoichiometric air / fuel mixture operated internal combustion engines, which is characterized in that the exhaust gas is passed through a particulate filter according to the invention.
  • the exhaust gas can be passed through a particulate filter according to the invention so that it enters the particulate filter through the channels E and exits through channels A again.
  • Particle filter enters and leaves it through channels E again.
  • FIG. 1 shows a particle filter according to the invention comprising a wall-flow filter of length L (1) with channels E (2) and channels A (3) extending in parallel between a first end (4) and a second end (5) of the wall-flow filter and which are separated by porous walls (6) forming surfaces OE (7) and OA (8), respectively, and wherein the channels E (2) at the second end (5) and the channels A (3) at the first end (4 ) are closed.
  • Coating Z (9) is located in the porous walls (6).
  • each ceramic wall flow filter made of highly porous cordierite with a diameter of 11.84 cm and a length of 15.24 cm and a cell density of 300 cpsi (46.5 cells per cm 2 ) and a wall thickness of 8.5 mil, ie 0.02 mm used.
  • Each filter was provided with a coating of 76.27 g / l based on the filter volume.
  • Alumina stabilized with lanthana was combined with an oxygen storage component containing 40% by weight of ceria, 50% by weight.
  • Alumina to oxygen storage component was 30:70.
  • the resulting suspension was then treated with continuous stirring with a palladium nitrate solution and a rhodium nitrate solution.
  • the resulting coating suspension was used directly for coating a commercially available wall flow filter substrate, wherein the
  • Rhodium of 5 1.
  • the coated filter thus obtained was dried and then calcined.
  • Alumina stabilized with lanthana was combined with an oxygen storage component containing 24% by weight of ceria, 60% by weight.
  • Alumina to oxygen storage component was 30:70.
  • the suspension thus obtained was subsequently stirred with continuous stirring a palladium nitrate solution and a rhodium nitrate solution.
  • the resulting coating suspension was used directly for coating a commercially available wall flow filter substrate, wherein the
  • Alumina stabilized with lanthana was combined with a first oxygen storage component comprising 40% by weight of ceria, 50% by weight of zirconia, 5% by weight of lanthana and 5% by weight of praseodymium oxide, and a second oxygen storage component containing 24% by weight.
  • Oxygen storage components were used in equal parts.
  • the weight ratio of alumina to oxygen storage components was 30:70.
  • the suspension thus obtained was then under constant stirring with a palladium nitrate solution and a
  • Wall flux filter substrate used, wherein the coating over 100% of the substrate length was introduced into the porous filter wall.
  • Comparative Example 1 Comparative Example 2 and Example 1 were aged in an engine test bench aging.
  • the aging consists of a fuel cut-off aging with 950 ° C exhaust gas temperature before the catalyst inlet (maximum bed temperature 1030 ° C).
  • Table 1 contains the temperatures Tso at which 50% of the considered component is converted in each case. It was the
  • Example 1 shows a marked improvement in the dynamic CO / NOx conversion after aging, while the
  • the stored oxygen quantity is calculated from the delay time of the post-catalytic lambda probe in relation to the pre-catalyst lambda probe.
  • Table 3 Static oxygen storage ability after aging for Example 1 and Comparative Examples 1 and 2
  • the dynamic oxygen storage capacity is determined.
  • the exhaust gas is subjected to various 1 amplitudes at a frequency of 1 Hz.
  • the amplitude signal of the Nachkat lambda probe is determined by the
  • the example according to the invention shows both a high static and a very good dynamic oxygen storage capacity after aging.

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  • Chemical & Material Sciences (AREA)
  • Engineering & Computer Science (AREA)
  • Chemical Kinetics & Catalysis (AREA)
  • Combustion & Propulsion (AREA)
  • Materials Engineering (AREA)
  • Health & Medical Sciences (AREA)
  • Organic Chemistry (AREA)
  • Mechanical Engineering (AREA)
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  • Ceramic Engineering (AREA)
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  • Exhaust Gas Treatment By Means Of Catalyst (AREA)

Abstract

La présente invention concerne un filtre à particules servant à éliminer les particules, le monoxyde de carbone, les hydrocarbures et les oxydes d'azote présents dans les gaz d'échappement de moteurs à combustion interne fonctionnant avec un mélange air/carburant stœchiométrique. Ce filtre à particules comprend un filtre à effet wall-flow de longueur L et un revêtement Z, le filtre à effet wall-flow comportant des conduits E et A qui s'étendent parallèlement entre une première et une deuxième extrémité du filtre à effet wall-flow et qui sont séparés par des parois poreuses qui forment des surfaces OE et OA, respectivement, les conduits E étant fermés au niveau de la deuxième extrémité et les conduits A au niveau de la première extrémité. L'invention se caractérise en ce que le revêtement Z se trouve dans les parois poreuses et s'étend à partir de la première extrémité du filtre à effet wall-flow sur toute la longueur L et contient de l'oxyde d'aluminium actif, deux oxydes mixtes de cérium/zirconium/métaux de terres rares différents l'un de l'autre et au moins un métal du groupe du platine.
EP18816073.3A 2017-12-19 2018-12-14 Filtre à particules à activité catalytique Active EP3727653B1 (fr)

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EP23212574.0A Pending EP4365421A3 (fr) 2017-12-19 2018-12-14 Filtre à particules à activité catalytique
EP18826640.7A Pending EP3727655A1 (fr) 2017-12-19 2018-12-19 Pot catalytique à trois voies monocouche
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CN111491715A (zh) 2020-08-04
US20230285899A1 (en) 2023-09-14
CN111511469A (zh) 2020-08-07
EP3727654A1 (fr) 2020-10-28
CN111491714B (zh) 2023-02-10
CN111491714A (zh) 2020-08-04
EP3501648B1 (fr) 2023-10-04
CN111511469B (zh) 2023-07-04
EP4365421A3 (fr) 2024-05-22
EP3727653B1 (fr) 2024-02-14
WO2019121995A1 (fr) 2019-06-27
CN111491715B (zh) 2022-12-27
US11179676B2 (en) 2021-11-23
EP3501648A1 (fr) 2019-06-26
US20200306693A1 (en) 2020-10-01
US11628400B2 (en) 2023-04-18
US11185820B2 (en) 2021-11-30
CN115990408A (zh) 2023-04-21
EP4365421A2 (fr) 2024-05-08
US20210079822A1 (en) 2021-03-18
WO2019121372A1 (fr) 2019-06-27
CN111511457A (zh) 2020-08-07
US20210069678A1 (en) 2021-03-11
EP3727655A1 (fr) 2020-10-28
US20210086135A1 (en) 2021-03-25
US11291952B2 (en) 2022-04-05
WO2019121375A1 (fr) 2019-06-27
WO2019121994A1 (fr) 2019-06-27

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